Cleavage of lignin C-O bonds over a heterogeneous rhenium catalyst through hydrogen transfer reactions

doi:10.1039/c9gc01710k

	Cleavage of lignin C-O bonds over a heterogeneous rhenium catalyst through hydrogen transfer reactions
	Zhang, Bo 2; Qi, Zaojuan 2; Li, Xinxin 2; Ji, Jianwei 1; Zhang, Leitei 2; Wang, Hua 2; Liu, Xiaoyan 2; Li, Changzhi 2,3
刊名	GREEN CHEMISTRY
	2019-10-21
卷号	21 期号:20 页码:5556-5564
ISSN号	1463-9262
DOI	10.1039/c9gc01710k
通讯作者	Li, Changzhi(licz@dicp.ac.cn)
英文摘要	Hydrogenolysis is one of the most popular strategies applied in the depolymerization of lignin for the production of aromatic chemicals. Currently, this strategy is mainly conducted under high hydrogen pressure, which can pose safety risks and is not sustainable and economical. Herein, we reported that heterogeneous rhenium oxide supported on active carbon (ReOx/AC) exhibited excellent activity in the selective cleavage of lignin C-O bonds in isopropanol. High yields of monophenols (up to 99.0%) from various lignin model compounds and aromatic liquid oils (>50%) from lignin feedstock were obtained under mild conditions in the absence of H-2. The characterization of the catalyst by X-ray absorption fine structure, X-ray photoelectron spectroscopy and H-2-temperature-programed reduction suggested that the activity of ReOx/AC could be attributed to the presence of ReIV-VI. The interaction between the surface oxygen groups of the active carbon and rhenium oxide could also play an important role in the cleavage of the C-O bonds. Notably, an ReOx/AC-catalyzed C-O bond cleavage pathway beyond a typical deoxydehydration mechanism was disclosed. More importantly, 2D-HSQC-NMR and GPC characterizations showed that ReOx/AC exhibited high activity not only in beta-O-4 cleavage, but also in the deconstruction of more resistant beta-5 and beta-beta linkages in lignin without destroying the aromatic ring. This study paves the way for the development of rhenium-based catalysts for the controlled reductive valorization of realistic lignin materials through a hydrogen transfer pathway.
资助项目	National Natural Science Foundation of China[21878288] ; National Natural Science Foundation of China[21690080] ; National Natural Science Foundation of China[21690083] ; DNL Cooperation Fund CAS[DNL180302] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDB17020100] ; National Key Projects for Fundamental Research and Development of China[2016YFA0202801]
WOS关键词	SELECTIVE CLEAVAGE ; PHENOLIC-COMPOUNDS ; TUNGSTEN CARBIDE ; MODEL COMPOUNDS ; WOODY BIOMASS ; BIO-OIL ; METAL ; DEPOLYMERIZATION ; DEOXYDEHYDRATION ; VALORIZATION
WOS研究方向	Chemistry ; Science & Technology - Other Topics
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000490291800008
资助机构	National Natural Science Foundation of China ; National Natural Science Foundation of China ; DNL Cooperation Fund CAS ; DNL Cooperation Fund CAS ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; National Key Projects for Fundamental Research and Development of China ; National Key Projects for Fundamental Research and Development of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DNL Cooperation Fund CAS ; DNL Cooperation Fund CAS ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; National Key Projects for Fundamental Research and Development of China ; National Key Projects for Fundamental Research and Development of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DNL Cooperation Fund CAS ; DNL Cooperation Fund CAS ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; National Key Projects for Fundamental Research and Development of China ; National Key Projects for Fundamental Research and Development of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DNL Cooperation Fund CAS ; DNL Cooperation Fund CAS ; Strategic Priority Research Program of the Chinese Academy of Sciences ; Strategic Priority Research Program of the Chinese Academy of Sciences ; National Key Projects for Fundamental Research and Development of China ; National Key Projects for Fundamental Research and Development of China
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/172556]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Li, Changzhi
作者单位	1.Shaanxi Univ Technol, Sch Chem & Environm Sci, Shaanxi Key Lab Catalysis, 1 Dongyihuan Rd, Hangzhou 723001, Zhejiang, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Thcluzol Appl Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China 3.Dalian Natl Lab Clean Energy, 457 Zhongshan Rd, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Zhang, Bo,Qi, Zaojuan,Li, Xinxin,et al. Cleavage of lignin C-O bonds over a heterogeneous rhenium catalyst through hydrogen transfer reactions[J]. GREEN CHEMISTRY,2019,21(20):5556-5564.
APA	Zhang, Bo.,Qi, Zaojuan.,Li, Xinxin.,Ji, Jianwei.,Zhang, Leitei.,...&Li, Changzhi.(2019).Cleavage of lignin C-O bonds over a heterogeneous rhenium catalyst through hydrogen transfer reactions.GREEN CHEMISTRY,21(20),5556-5564.
MLA	Zhang, Bo,et al."Cleavage of lignin C-O bonds over a heterogeneous rhenium catalyst through hydrogen transfer reactions".GREEN CHEMISTRY 21.20(2019):5556-5564.